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A highly selective FER-based catalyst to produce n-butenes from isobutanol
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-11-25 , DOI: 10.1016/j.apcatb.2020.119699
Stijn Van Daele , Delphine Minoux , Nikolai Nesterenko , Sylvie Maury , Vincent Coupard , Valentin Valtchev , Arnaud Travert , Jean-Pierre Gilson

The conversion of isobutanol to light olefins over zeolites was investigated by IR operando spectroscopy. FER zeolites showed a surprisingly high selectivity for the direct conversion of iso-butanol to linear butenes, hence catalyzing dehydration and skeletal isomerization in one step. As a fundamental understanding of the separate reactions is required to design superior catalysts, an in-situ and operando FT-IR mechanistic study of the reaction was carried out. The spectroscopic data, the derived species participating and their respective role are analyzed using chemometric (PCA and MCR-ALS) tools. We highlighted the role played by the external acid sites and the requirement of a specific distance between these sites to ensure the n-butene selectivity and point that the internal Brønsted acidity has an adverse effect on the catalyst stability. Moreover, there is no correlation between the carbon species formed on the surface and the exceptional selectivity towards n-butenes, allowing to exclude a “carbon pool” mechanism.



中文翻译:

一种高选择性的基于FER的催化剂,可从异丁醇生产正丁烯

通过IR操作光谱法研究了异丁醇在沸石上的转化为轻质烯烃。FER沸石对异丁醇直接转化为线性丁烯具有惊人的高选择性,因此一步催化了脱水和骨架异构化。作为对单独反应的基本了解,需要设计出色的催化剂,原位和操作催化剂对该反应进行了FT-IR机理研究。使用化学计量学(PCA和MCR-ALS)工具分析光谱数据,参与的物种及其各自的作用。我们着重指出了外部酸性位点所起的作用,以及这些位点之间必须有特定距离以确保正丁烯选择性,并指出内部布朗斯台德酸度对催化剂稳定性有不利影响。此外,表面上形成的碳物种与对正丁烯的优异选择性之间没有关联,从而排除了“碳库”机制。

更新日期:2020-12-09
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